Evidence for d-wave superconductivity of infinite-layer nickelates from low-energy electrodynamics.

The discovery of superconductivity in infinite-layer nickelates established another category of unconventional superconductors that shares structural and electronic similarities with cuprates. However, key issues of the superconducting pairing symmetry, gap amplitude and superconducting fluctuations are yet to be addressed. Here we utilize static and ultrafast terahertz spectroscopy to address these. We demonstrate that the equilibrium terahertz conductivity and non-equilibrium terahertz responses of an optimally Sr-doped nickelate film (superconducting transition temperature of Tc = 17 K) are in line with the electrodynamics of d-wave superconductivity in the dirty limit. The gap-to-Tc ratio (2Δ/kBTc) is found to be 3.4, indicating that the superconductivity falls in the weak coupling regime. In addition, we observed substantial superconducting fluctuations near Tc that do not extend into the deep normal state as the optimally hole-doped cuprates do. Our results support a d-wave system that closely resembles the electron-doped cuprates.

Chirality manipulation of ultrafast phase switches in a correlated CDW-Weyl semimetal.

Light engineering of correlated states in topological materials provides a new avenue of achieving exotic topological phases inaccessible by conventional tuning methods. Here we demonstrate a light control of correlation gaps in a model charge-density-wave (CDW) and polaron insulator (TaSe4)2I recently predicted to be an axion insulator. Our ultrafast terahertz photocurrent spectroscopy reveals a two-step, non-thermal melting of polarons and electronic CDW gap via the fluence dependence of a longitudinal circular photogalvanic current. This helicity-dependent photocurrent reveals continuous ultrafast phase switches from the polaronic state to the CDW (axion) phase, and finally to a hidden Weyl phase as the pump fluence increases. Additional distinctive attributes aligning with the light-induced switches include: the mode-selective coupling of coherent phonons to the polaron and CDW modulation, and the emergence of a non-thermal chiral photocurrent above the pump threshold of CDW-related phonons. The demonstrated ultrafast chirality control of correlated topological states here holds large potentials for realizing axion electrodynamics and advancing quantum-computing applications.

Study of Elastic and Structural Properties of BaFe2As2 Ultrathin Film Using Picosecond Ultrasonics.

We obtain the through-thickness elastic stiffness coefficient (C33) in nominal 9 nm and 60 nm BaFe2As2 (Ba-122) thin films by using picosecond ultrasonics. Particularly, we reveal the increase in elastic stiffness as film thickness decreases from bulk value down to 9 nm, which we attribute to the increase in intrinsic strain near the film-substrate interface. Our density functional theory (DFT) calculations reproduce the observed acoustic oscillation frequencies well. In addition, temperature dependence of longitudinal acoustic (LA) phonon mode frequency for 9 nm Ba-122 thin film is reported. The frequency change is attributed to the change in Ba-122 orthorhombicity (a-b)/(a+b). This conclusion can be corroborated by our previous ultrafast ellipticity measurements in 9 nm Ba-122 thin film, which exhibit strong temperature dependence and indicate the structural phase transition temperature Ts.

A light-induced phononic symmetry switch and giant dissipationless topological photocurrent in ZrTe5.

Dissipationless currents from topologically protected states are promising for disorder-tolerant electronics and quantum computation. Here, we photogenerate giant anisotropic terahertz nonlinear currents with vanishing scattering, driven by laser-induced coherent phonons of broken inversion symmetry in a centrosymmetric Dirac material ZrTe5. Our work suggests that this phononic terahertz symmetry switching leads to formation of Weyl points, whose chirality manifests in a transverse, helicity-dependent current, orthogonal to the dynamical inversion symmetry breaking axis, via circular photogalvanic effect. The temperature-dependent topological photocurrent exhibits several distinct features: Berry curvature dominance, particle-hole reversal near conical points and chirality protection that is responsible for an exceptional ballistic transport length of ~10 µm. These results, together with first-principles modelling, indicate two pairs of Weyl points dynamically created by B1u phonons of broken inversion symmetry. Such phononic terahertz control breaks ground for coherent manipulation of Weyl nodes and robust quantum transport without application of static electric or magnetic fields.

Biexcitons in monolayer transition metal dichalcogenides tuned by magnetic fields.

We present time-integrated four-wave mixing measurements on monolayer MoSe2 in magnetic fields up to 25 T. The experimental data together with time-dependent density function theory calculations provide interesting insights into the biexciton formation and dynamics. In the presence of magnetic fields the coherence at negative and positive time delays is dominated by intervalley biexcitons. We demonstrate that magnetic fields can serve as a control to enhance the biexciton formation and help search for more exotic states of matter, including the creation of multiple exciton complexes and excitonic condensates.

Ultrafast terahertz snapshots of excitonic Rydberg states and electronic coherence in an organometal halide perovskite.

How photoexcitations evolve into Coulomb-bound electron and hole pairs, called excitons, and unbound charge carriers is a key cross-cutting issue in photovoltaics and optoelectronics. Until now, the initial quantum dynamics following photoexcitation remains elusive in the hybrid perovskite system. Here we reveal excitonic Rydberg states with distinct formation pathways by observing the multiple resonant, internal quantum transitions using ultrafast terahertz quasi-particle transport. Nonequilibrium emergent states evolve with a complex co-existence of excitons, carriers and phonons, where a delayed buildup of excitons under on- and off-resonant pumping conditions allows us to distinguish between the loss of electronic coherence and hot state cooling processes. The nearly ∼1 ps dephasing time, efficient electron scattering with discrete terahertz phonons and intermediate binding energy of ∼13.5 meV in perovskites are distinct from conventional photovoltaic semiconductors. In addition to providing implications for coherent energy conversion, these are potentially relevant to the development of light-harvesting and electron-transport devices.

Ultrafast observation of critical nematic fluctuations and giant magnetoelastic coupling in iron pnictides.

Many of the iron pnictides have strongly anisotropic normal-state characteristics, important for the exotic magnetic and superconducting behaviour these materials exhibit. Yet, the origin of the observed anisotropy is unclear. Electronically driven nematicity has been suggested, but distinguishing this as an independent degree of freedom from magnetic and structural orders is difficult, as these couple together to break the same tetragonal symmetry. Here we use time-resolved polarimetry to reveal critical nematic fluctuations in unstrained Ba(Fe1-xCox)2As2. The femtosecond anisotropic response, which arises from the two-fold in-plane anisotropy of the complex refractive index, displays a characteristic two-step recovery absent in the isotropic response. The fast recovery appears only in the magnetically ordered state, whereas the slow one persists in the paramagnetic phase with a critical divergence approaching the structural transition temperature. The dynamics also reveal a gigantic magnetoelastic coupling that far exceeds electron-spin and electron-phonon couplings, opposite to conventional magnetic metals.

Femtosecond switching of magnetism via strongly correlated spin-charge quantum excitations.

The technological demand to push the gigahertz (10(9) hertz) switching speed limit of today's magnetic memory and logic devices into the terahertz (10(12) hertz) regime underlies the entire field of spin-electronics and integrated multi-functional devices. This challenge is met by all-optical magnetic switching based on coherent spin manipulation. By analogy to femtosecond chemistry and photosynthetic dynamics--in which photoproducts of chemical and biochemical reactions can be influenced by creating suitable superpositions of molecular states--femtosecond-laser-excited coherence between electronic states can switch magnetic order by 'suddenly' breaking the delicate balance between competing phases of correlated materials: for example, manganites exhibiting colossal magneto-resistance suitable for applications. Here we show femtosecond (10(-15) seconds) photo-induced switching from antiferromagnetic to ferromagnetic ordering in Pr0.7Ca0.3MnO3, by observing the establishment (within about 120 femtoseconds) of a huge temperature-dependent magnetization with photo-excitation threshold behaviour absent in the optical reflectivity. The development of ferromagnetic correlations during the femtosecond laser pulse reveals an initial quantum coherent regime of magnetism, distinguished from the picosecond (10(-12) seconds) lattice-heating regime characterized by phase separation without threshold behaviour. Our simulations reproduce the nonlinear femtosecond spin generation and underpin fast quantum spin-flip fluctuations correlated with coherent superpositions of electronic states to initiate local ferromagnetic correlations. These results merge two fields, femtosecond magnetism in metals and band insulators, and non-equilibrium phase transitions of strongly correlated electrons, in which local interactions exceeding the kinetic energy produce a complex balance of competing orders.